Controlled Doping in Graphene Monolayers by Trapping Organic Molecules at the Graphene–Substrate Interface

We report controlled doping in graphene monolayers through charge-transfer interaction by trapping selected organic molecules between graphene and underneath substrates. Controllability has been demonstrated in terms of shifts in Raman peaks and Dirac points in graphene monolayers. Under field effect transistor geometry, a shift in the Dirac point to the negative (positive) gate voltage region gives an inherent signature of n- (p-)type doping as a consequence of charge-transfer interaction between organic molecules and graphene. The proximity of organic molecules near the graphene surface as a result of trapping is evidenced by Raman and infrared spectroscopies. Density functional theory calculations corroborate the experimental results and also indicate charge-transfer interaction between certain organic molecules and graphene sheets resulting p- (n-)type doping and reveals the donor and acceptor nature of molecules. Interaction between molecules and graphene has been discussed in terms of calculated Mulliken charge-transfer and binding energy as a function of optimized distance.